Synergistic effect of the metal-support interaction and interfacial oxygen vacancy for CO_(2) hydrogenation to methanol over Ni/In_(2)O_(3) catalyst:A theoretical study

Indium oxide supported nickel catalyst has been experimentally confirmed to be highly active for CO_(2) hydrogenation towards methanol.In this work,the reaction mechanism for CO_(2) hydrogenation to methanol has been investigated on a model Ni/In_(2)O_(3) catalyst,i.e.,Ni_(4)/In_(2)O_(3),via the density functional theory(DFT)study.Three possible reaction pathways,i.e.,the formate pathway,CO hydrogenation and the reverse water-gas-shift(RWGS)pathways,have been examined on this model catalyst.It has been demonstrated that the RWGS pathway is the most theoretically-favored for CO_(2) hydrogenation to methanol.The complete RWGS pathway follows CO_(2)+6 H→COOH+5 H→CO+H_(2)O+4 H→HCO+H_(2)O+3 H→H_(2)CO+H_(2)O+2 H→H_(3)CO+H_(2)O+H→H_(3)COH+H_(2) O.Furthermore,it has been also proved that the interfacial oxygen vacancy can serve as the active site for boosting the CO_(2) adsorption and charge transfer between the nickel species and indium oxide,which synergistically promotes the consecutive CO_(2) hydrogenation towards methanol.

The feasibility study of the indium oxide supported silver catalyst for selective hydrogenation of CO_(2)to methanol

Silver catalyst has been extensively investigated for photocatalytic and electrochemical CO_(2) reduction.However,its high activity for selective hydrogenation of CO_(2) to methanol has not been confirmed.Here,the feasibility of the indium oxide supported silver catalyst was investigated for CO_(2) hydrogenation to methanol by the density functional theoretical(DFT)study and then by the experimental investigation.The DFT study shows there exists an intense Ag-In_(2)O_(3) interaction,which causes silver to be positively charged.The positively charged Ag species changes the electronic structure of the metal,facilitates the formation of the Ag-In_(2)O_(3) interfacial site for activation and dissociation of carbon dioxide.The promoted CO_(2) dissociation leads to the enhanced methanol synthesis via the CO hydrogenation route as CO_(2)^(*)→CO^(*)→HCO^(*)→H_(2)CO^(*)→H_(3)CO^(*)→H_(3)COH^(*).The Ag/In_(2)O_(3)catalyst was then prepared using the deposition-precipitation method.The experimental study confirms the theoretical prediction.The methanol selectivity of CO_(2) hydrogenation on Ag/In_(2)O_(3) reaches 100.0%at reaction temperature of 200℃.It remains more than 70.0%between 200 and 275℃.At 300℃and 5 MPa,the methanol selectivity still keeps 58.2%with a CO_(2) conversion of 13.6%and a space-time yield(STY)of methanol of 0.453 g_(methanol)g_(cat)^(-1)h^(-1),which is the highest methanol STY ever reported for silver catalyst.The catalyst characterization confirms the intense Ag-In_(2)O_(3)interaction as well,which causes high Ag dispersion,increases and stabilizes the oxygen vacancies and creates the active Ag-In_(2)O_(3)interfacial site for the enhanced CO_(2)hydrogenation to methanol.

Characteristics of DBD micro-discharge at different pressure and its effect on the performance of oxygen plasma reactor

The oxygen plasma reactor based on dielectric barrier discharge principle can produce a high concentration of reactive oxygen species,which can cooperate with hydraulic cavitation gas-liquid mixer to realize the application of advanced oxidation technology in water treatment.In this technology,the work pressure of the oxygen plasma reactor is decreased by the vacuum suction effect generated in the snap-back section of the gas-liquid mixed container.In this paper,the characteristics of single micro-discharge at different pressures were investigated with the methods of discharge image,electrical characteristics and spectral diagnosis,in order to analyze the electrical characteristics and reactive oxygen species generation efficiency of oxygen plasma reactor at the pressure range from 60 kPa to 100 kPa.The study indicated that,when the pressure decreases,the duty ratio of ionization in the discharge gap and number of electrons with high energy increases,leading to a rise in reactive oxygen species production.When the oxygen reaches the maximum ionization,the concentration of reactive oxygen species is the highest.Then,the discharge intensity continues to increase,producing more heat,which will decompose the ozone and lower the production of reactive oxygen species.The oxygen plasma reactor has an optimum working pressure at different input powers,which makes the oxygen plasma reactor the most efficient in generating reactive oxygen species.

Research on resonance parameters matching based on partitioned operation method of atmospheric pressure plasma reactor array

Matching optimization of resonant parameters among the high power inverters,low power transformers and plasma reactors have significant effects on the performance and output of the reactor array when applying the partitioned operation method.In this paper,the Matlab/Simulink electrical model was established based on the method of partitioned operation.The matching relation between resonant parameters is analyzed on the basis of experimental result.As a consequence,transformer leakage inductance and working frequency are the important parameters influencing the operational efficiency of system,leakage inductance of transformer should be adjusted based on the equivalent capacitance of plasma reactor to realize the matching optimization of resonant parameters.

Charge storage coating based triboelectric nanogenerator and its applications in self-powered anticorrosion and antifouling

As a novel energy-harvesting device,a triboelectric nanogenerator(TENG)can harvest almost all mechanical energy and transform it into electrical energy,but its output is low.Although the micro-nano structures of triboelectrode surfaces can improve their output efficiency,they lead to high costs and are not suitable for large-scale applications.To address this problem,we developed a novel TENG coating with charge-storage properties.In this study,we modified an acrylic resin,a friction material,with nano-BaTiO_(3) particles and gas phase fluorination.The charge-trapping ability of nanoparticles was used to improve the output of TENG.The short-circuit current and the output voltage of coating-based TENGs featuring charge storage and electrification reached 15μA and 800 V,respectively,without decay for longtime working.On this basis,self-powered anticorrosion and antifouling systems are designed to reduce the open circuit potential of A3 steel by 510 mV and reduce the adhesion rate of algae on the surface of metal materials.This study presents a high-output,stable,coating-based TENG with potential in practical applications for anticorrosion and antifouling.

Noise-sidebands-free and ultra-low-RIN 1.5 μm single-frequency fiber laser towards coherent optical detection

A noise-sidebands-free and ultra-low relative intensity noise(RIN) 1.5 μm single-frequency fiber laser is demonstrated for the first time to our best knowledge. Utilizing a self-injection locking framework and a booster optical amplifier, the noise sidebands with relative amplitudes as high as 20 dB are completely suppressed.The RIN is remarkably reduced by more than 64 dB at the relaxation oscillation peak to retain below-150 dB∕Hz in a frequency range from 75 kHz to 50 MHz, while the quantum noise limit is -152.9 d B∕Hz.Furthermore, a laser linewidth narrower than 600 Hz, a polarization-extinction ratio of more than 23 dB, and an optical signal-to-noise ratio of more than 73 dB are acquired simultaneously. This noise-sidebands-free and ultralow-RIN single-frequency fiber laser is highly competitive in advanced coherent light detection fields including coherent Doppler wind lidar, high-speed coherent optical communication, and precise absolute distance coherent measurement.

Isolated zinc in mordenite stabilizing carbonylation of dimethyl ether to methyl acetate

Herein, we prepared a series of H-Zn-mordenite (H-Zn-MOR) catalysts by adding zinc source into the initial sols during the synthesis of mordenite (MOR). The results indicated that isolated Zn ions were highly dispersed in the catalysts. The addition of zinc led to the increase of Si/Al in the framework of MOR,the change of the distribution of acid sites and the change of acid strength. We investigated the catalytic performance of the H-Zn-MOR catalysts and the HMOR catalysts for carbonylation of dimethyl ether to methyl acetate. The addition of zinc improved the catalytic performance and made the drop of the conversion over the Zn-0.003 and Zn-0.005 catalysts to be about the half of that over the HMOR catalyst.We attributed it to the change of the acid properties, which further change the rate of coke deposition.

CO_(2) hydrogenation to methanol over Rh/In_(2)O_(3)–ZrO_(2)catalyst with improved activity

The In_(2)O_(3)supported rhodium catalyst has been previously confirmed to be active for CO_(2)hydrogenation to methanol.In this work,the In_(2)O_(3)–ZrO_(2)solid solution was prepared and employed to support the rhodium catalyst.The deposition-precipitation method was applied to make the Rh catalyst highly dispersed.The catalyst characterization confirms that the use of ZrO_(2)optimizes and stabilizes the oxygen vacancies of In_(2)O_(3),which causes the enhanced adsorption and activation of CO_(2).The highly dispersed Rh catalyst remarkably improves the hydrogenation ability of the In_(2)O_(3)–ZrO_(2)support.Compared to Rh/In_(2)O_(3),the In_(2)O_(3)–ZrO_(2)supported Rh catalyst shows significantly higher activity with high methanol selectivity.For instance,at 300℃ and 5 MPa,the methanol selectivity over Rh/In_(2)O_(3)–ZrO_(2)reaches 66.5%with a space-time yield(STY)of methanol of 0.684 g MeOH h^(-1) g cat-1 and a CO_(2)conversion of 18.1%.The methanol selectivity and methanol STY at 300℃ is 19% and 26% higher than that of the Rh/In_(2)O_(3)catalyst.

A monotonicity theorem and its applications to weighted elliptic equations

We study the equation wtt + ?SN-1w-μwt-δw + h(t, ω)wp= 0,(t, ω) ∈ R × SN-1, and under some conditions we prove a monotonicity theorem for its positive solutions. Applying this monotonicity theorem,we obtain a Liouville-type theorem for some nonlinear elliptic weighted singular equations. Moreover, we obtain the necessary and sufficient condition for-div(|x|θ▽u) = |x|lup, x ∈ RN\{0} having positive solutions which are bounded near 0, which is also a positive answer to Souplet’s conjecture(see Phan and Souplet(2012)) on the weighted Lane-Emden equation-?u = |x|aup, x ∈ RN.